From the paths you've described above, I have a feeling that the TestSpecs.xls file is a resource that belongs to an assembly being referenced by the test project (rather than being a resource owned by the test project itself), is this the case?
NCrunch will separate components from each other in its workspaces (under AppData\Local ...). This can be a problem where built assemblies depend upon resources that are normally found adjacent to other assemblies that they reference, as the test application domain is wired together artificially by NCrunch and doesn't necessarily follow the same structure as the solution you have open in Visual Studio.
There's a
detailed explanation of this situation in the documentation, along with some suggestions on how you can solve the problem. The 'quick fix' is to turn on the 'Copy referenced assemblies to workspace' configuration option for the projects that are involved, though I recommend this only as a last resort, as it will greatly elevate your build times. A much better option is to try and find the TestSpecs.xls file by using the location of the assembly that owns it, i.e. Path.GetDirectoryName(typeof(classWithinAssemblyOwningTestSpecsXlsFile).Assembly.Location) + "\Services\TestSpecs.xls"